Disclosed is a method of manufacturing a multilayer zirconia block for artificial teeth, including a first material mixing step of mixing a 3 mol % yttrium oxide-tetragonal zirconia polycrystal and an organic binder, a second material mixing step of mixing a 3 mol % yttrium oxide-tetragonal zirconia polycrystal, a 5 mol % yttrium oxide-tetragonal zirconia polycrystal and an organic binder, a third material mixing step of mixing a 5 mol % yttrium oxide-tetragonal zirconia polycrystal and an organic binder, a compression molding step of sequentially placing the mixtures obtained in the first material mixing step, the second material mixing step, and the third material mixing step in a mold for compression molding and performing compression molding, and a calcination step of calcining a compression molded product obtained in the compression molding step. This method provides a multilayer zirconia block that contains yttrium oxide, the amount of which is adjusted in the manufacturing process, thus showing a color similar to that of natural teeth after impregnation with a coloring solution.